Title: Synthesis and sintering of UN-UO 2 fuel composites

In this study, the design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO 2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO 2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized from elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO 2 in a planetary ball mill. UN and UN – UO 2 composite pellets were sintered in Ar – (0–1 at%) N 2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO 2 composite pellets were also sintered in Ar – 100 ppm N 2 to assess the effects of temperature (1700–2000 °C) on the final grain morphology and phase concentration.

@article{osti_1294431,
title = {Synthesis and sintering of UN-UO2 fuel composites},
author = {Jaques, Brian J. and Watkins, Jennifer and Croteau, Joseph R. and Alanko, Gordon A. and Tyburska-Puschel, Beata and Meyer, Mitch and Xu, Peng and Lahoda, Edward J. and Butt, Darryl P.},
abstractNote = {In this study, the design and development of an economical, accident tolerant fuel (ATF) for use in the current light water reactor (LWR) fleet is highly desirable for the future of nuclear power. Uranium mononitride has been identified as an alternative fuel with higher uranium density and thermal conductivity when compared to the benchmark, UO2, which could also provide significant economic benefits. However, UN by itself reacts with water at reactor operating temperatures. In order to reduce its reactivity, the addition of UO2 to UN has been suggested. In order to avoid carbon impurities, UN was synthesized from elemental uranium using a hydride-dehydride-nitride thermal synthesis route prior to mixing with up to 10 wt% UO2 in a planetary ball mill. UN and UN – UO2 composite pellets were sintered in Ar – (0–1 at%) N2 to study the effects of nitrogen concentration on the evolved phases and microstructure. UN and UN-UO2 composite pellets were also sintered in Ar – 100 ppm N2 to assess the effects of temperature (1700–2000 °C) on the final grain morphology and phase concentration.},
doi = {10.1016/j.jnucmat.2015.06.029},
journal = {Journal of Nuclear Materials},
number = C,
volume = 466,
place = {United States},
year = {2015},
month = {6}
}

Uranium mononitride (UN) is important as a nuclear fuel. Fabrication of UN in its microspherical form also has its own merits since the advent of the concept of accident-tolerant fuel, where UN is being considered as a potential fuel in the form of TRISO particles. But, not many processes have been well established to synthesize kernels of UN. Therefore, a process for synthesis of microspherical UN with a minimum amount of carbon is discussed herein. First, a series of single-phased microspheres of uranium sesquinitride (U 2N 3) were synthesized by nitridation of UO 2+C microspheres at a few different temperatures.more » Resulting microspheres were of low-density U 2N 3 and decomposed into low-density UN. The variation of density of the synthesized sesquinitrides as a function of its chemical composition indicated the presence of extra (interstitial) nitrogen atoms corresponding to its hyperstoichiometry, which is normally indicated as α-U 2N 3. Average grain sizes of both U 2N 3 and UN varied in a range of 1–2.5 μm. In addition, these had a considerably large amount of pore spacing, indicating the potential sinterability of UN toward its use as a nuclear fuel.« less

High uranium density composite fuels composed of UN and U 3Si 2 have been fabricated using a liquid phase sintering route at temperatures between 1873 K and 1973 K and spanning compositions of 10 vol% to 40 vol% U 3Si 2. Microstructural analysis and phase characterization revealed the formation of an U-Si-N phase of unknown structure. Microcracking was observed in the U-Si portion of the composite microstructure that likely originates from the mismatched coefficient of thermal expansion between the UN and U 3Si 2 leading to stresses on heating and cooling of the composite. Thermal expansion coefficient, thermal diffusivity, andmore » thermal conductivity were characterized for each of the compositions as a function of temperature to 1673 K. Hysteresis is observed in the thermal diffusivity for the 20 vol% through 40 vol% specimens between room temperature and 1273 K, which is attributed to the microcracking in the U-Si phase. Thermal conductivity of the composites was modeled using the MOOSE framework based on the collected microstructure data. In conclusion, the impact of irradiation on thermal conductivity was also simulated for this class of composite materials.« less

In this paper, flash sintering was demonstrated on stoichiometric and non-stoichiometric uranium dioxide pellets at temperatures ranging from room temperature (26°C) up to 600°C. The onset conditions for flash sintering were determined for three stoichiometries (UO 2.00, UO 2.08, and UO 2.16) and analyzed against an established thermal runaway model. The presence of excess oxygen was found to enhance the flash sintering onset behavior of uranium dioxide, lowering the field required to flash and shortening the time required for a flash to occur. Finally, the results from this study highlight the effect of stoichiometry on the flash sintering behavior ofmore » uranium dioxide and will serve as the foundation for future studies on this material.« less